Photon Antibunching in the Photoluminescence Spectra of a Single Carbon Nanotube

Högele, Alexander; Galland, Christophe; Winger, Martin; İmamoğlu, Ataç

doi:10.1103/physrevlett.100.217401

Cited by 254 publications

(301 citation statements)

References 39 publications

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“…Recent studies of fluorescence antibunching have confirmed that SWNTs are single-photon emitters at low temperatures. 80 For example, the probability that an SWNT will simultaneously emit more than one photon is only 3% up to 10 K, and increases only to 15% at 25 K. Antibunching behavior is more pronounced at low temperatures due to strong localization of excitons, which diminishes the strength of nonlinear interactions between different sites along the nanotube sidewall. 80 Although SWNT antibunching has not yet been observed at room temperature, if single photon emission could be demonstrated under these conditions, nanotubes would be leading candidates for development as quantum optical components.…”

Section: Discussionmentioning

confidence: 99%

“…80 Specifically, quantum cryptography requires a source of single photons, as sources that emit two or more photons provide opportunities for a compromised transmission. 81 SWNTs could be an exceptional source of single photons because they do not show fluorescence intermittency at room temperature, nor do they photobleach.…”

Section: Optical Properties and Applicationsmentioning

confidence: 99%

“…81 SWNTs could be an exceptional source of single photons because they do not show fluorescence intermittency at room temperature, nor do they photobleach. 80,84 However, the extremely low luminescence efficiency for SWNTs remains a major concern for all potential fluorescence-based applications. 77…”

Section: Optical Properties and Applicationsmentioning

confidence: 99%

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Photophysics of Individual Single-Walled Carbon Nanotubes

2008

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Single-walled carbon nanotubes (SWNTs) are cylindrical graphitic molecules that have remained at the forefront of nanomaterials research since 1991, largely due to their exceptional and unusual mechanical, electrical, and optical properties. The motivation for understanding how nanotubes interact with light (i.e., SWNT photophysics) is both fundamental and applied. Individual nanotubes may someday be used as superior near-infrared fluorophores, biological tags and sensors, and components for ultrahigh-speed optical communications systems. Establishing an understanding of basic nanotube photophysics is intrinsically significant and should enable the rapid development of such innovations. Unlike conventional molecules, carbon nanotubes are synthesized as heterogeneous samples, composed of molecules with different diameters, chiralities, and lengths. Because a nanotube can be either metallic or semiconducting depending on its particular molecular structure, SWNT samples are also mixtures of conductors and semiconductors. Early progress in understanding the optical characteristics of SWNTs was limited because nanotubes aggregate when synthesized, causing a mixing of the energy states of different nanotube structures. Recently, significant improvements in sample preparation have made it possible to isolate individual nanotubes, enabling many advances in characterizing their optical properties. In this Account, single-molecule confocal microscopy and spectroscopy were implemented to study the fluorescence from individual nanotubes. Single-molecule measurements naturally circumvent the difficulties associated with SWNT sample inhomogeneities. Intrinsic SWNT photoluminescence has a simple narrow Lorentzian line shape and a polarization dependence, as expected for a one-dimensional system. Although the local environment heavily influences the optical transition wavelength and intensity, single nanotubes are exceptionally photostable. In fact, they have the unique characteristic that their single molecule fluorescence intensity remains constant over time; SWNTs do not “blink” or photobleach under ambient conditions. In addition, transient absorption spectroscopy was used to examine the relaxation dynamics of photoexcited nanotubes and to elucidate the nature of the SWNT excited state. For metallic SWNTs, very fast initial recovery times (300–500 fs) corresponded to excited-state relaxation. For semiconducting SWNTs, an additional slower decay component was observed (50–100 ps) that corresponded to electron–hole recombination. As the excitation intensity was increased, multiple electron–hole pairs were generated in the SWNT; however, these e−h pairs annihilated each other completely in under 3 ps. Studying the dynamics of this annihilation process revealed the lifetimes for one, two, and three e−h pairs, which further confirmed that the photoexcitation of SWNTs produces not free electrons but rather one-dimensional bound electron–hole pairs (i.e., excitons). In summary, nanotube photophysics is a rapidly developing area o...

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Section: Discussionmentioning

confidence: 99%

Section: Optical Properties and Applicationsmentioning

confidence: 99%

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Photophysics of Individual Single-Walled Carbon Nanotubes

2008

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“…Our results can have important implications in SWNT-based photonics and quantum optics in the light of recent observations of exciton localization in SWNTs due to the presence of disorder. 99 …”

Section: Discussionmentioning

confidence: 99%

Modifying the electronic structure of semiconducting single-walled carbon nanotubes byAr+ion irradiation

et al. 2009

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Local controllable modification of the electronic structure of carbon nanomaterials is important for the development of carbon-based nanoelectronics. By combining density-functional theory simulations with Arion-irradiation experiments and low-temperature scanning tunneling microscopy and spectroscopy ͑STM/STS͒ characterization of the irradiated samples, we study the changes in the electronic structure of single-walled carbon nanotubes due to the impacts of energetic ions. As nearly all irradiation-induced defects look as nondistinctive hillocklike features in the STM images, we compare the experimentally measured STS spectra to the computed local density of states of the most typical defects with an aim to identify the type of defects and assess their abundance and effects on the local electronic structure. We show that individual irradiationinduced defects can give rise to single and multiple peaks in the band gap of the semiconducting nanotubes and that a similar effect can be achieved when several defects are close to each other. We further study the stability of defects and their evolution during STM measurements. Our results not only shed light on the abundance of the irradiation-induced defects in carbon nanotubes and their signatures in STS spectra but also suggest a way the STM can be used for engineering the local electronic structure of defected carbon nanotubes.

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“…2 Various schemes for single-photon generation 3 have been proposed, including two-photon down conversion using nonlinear crystals, 4 photon blockade 5 and fluorescence of single molecules, 6 trapped ions and atoms, 7 carbon nanotubes, 8 as well as diamond color centers. 9 Due to their versatility, scalability, and ease to handle, single semiconductor quantum dots (QDs) are amongst the most promising candidates of stable, solid-state emitters for such applications.…”

Section: Introductionmentioning

confidence: 99%

Controlling the properties of single photon emitters via the Purcell effect

et al. 2012

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Single photon emission by an InAs/GaAs quantum dot weakly coupled to a photonic crystal microcavity has been studied as a function of energy detuning. Precise and continuous control of the photon statistics as well as of the linear polarization emission angle is achieved simply by changing the energy detuning between the exciton and the cavity mode. A continuous decrease of the antibunching time, the bunching amplitude and the g 2 (0) value is observed as the detuning is decreased at constant excitation rate, due to the detuning-dependent Purcell effect.

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Photon Antibunching in the Photoluminescence Spectra of a Single Carbon Nanotube

Cited by 254 publications

References 39 publications

Photophysics of Individual Single-Walled Carbon Nanotubes

Photophysics of Individual Single-Walled Carbon Nanotubes

Modifying the electronic structure of semiconducting single-walled carbon nanotubes byAr+ion irradiation

Controlling the properties of single photon emitters via the Purcell effect

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